We report on the excitation of single molecules via narrow zero-phonon transitions using short laser pulses. By monitoring the Stokes-shifted fluorescence, we studied the excited state population as a function of the delay time, laser intensity, and frequency detuning. A pi-pulse excitation was demonstrated with merely 500 photons, and 5 Rabi cycles were achieved at higher excitation powers. Our findings are in good agreement with theoretical calculations and provide a first step toward coherent manipulation of the electronic states of single molecules with few photons.
Squeezed states of harmonic oscillators are a central resource for continuous-variable quantum sensing, computation and communication. Here we propose a method for the generation of very good approximations to highly squeezed vacuum states with low excess anti-squeezing using only a few oscillator-qubit coupling gates through a Rabi-type interaction Hamiltonian. This interaction can be implemented with several different methods, which has previously been demonstrated in superconducting circuit and trapped-ion platforms. The protocol is compatible with other protocols manipulating quantum harmo…
We use coherent excitation of 3-16 atom ensembles to demonstrate collective Rabi flopping mediated by Rydberg blockade. Using calibrated atom number measurements, we quantitatively confirm the expected $\sqrt{N}$ Rabi frequency enhancement to within 4%. The resulting atom number distributions are consistent with essentially perfect blockade. We then use collective Rabi $π$ pulses to produce ${\cal N}=1,2$ atom number Fock states with fidelities of 62% and 48% respectively. The ${\cal N}=2$ Fock state shows the collective Rabi frequency enhancement without corruption from atom number fluctuatio…
We show that the excitation probability of a state within a manifold of levels undergoes Rabi oscillations with frequency determined by the energy difference between the states and not by the pulse area for sufficiently strong pulses. The observed dynamics can be used as a procedure for robust state preparation as an alternative to adiabatic passage and as a useful spectroscopic method.
Dynamics of zeroth order quantum coherences and preparation of the pseudopure states in homonuclear systems of dipolar coupling spins is closely examined. It has been shown an extreme important role of the non-diagonal part of zeroth order coherence in construction of the pseudopure state. Simulations of the preparation process of pseudopure states with the real molecular structures (a rectangular (-chloro- -nitrobenzene molecule), a chain (hydroxyapatite molecule), a ring (benzene molecule), and a double ring (cyclopentane molecule)) open the way to experimental testing of the obtained result…
Cluster states, a special type of highly entangled states, are a universal resource for measurement-based quantum computation. Here, we propose an efficient one-step generation scheme for cluster states in semiconductor quantum dot molecules, where qubits are encoded on singlet and triplet state of two coupled quantum dots. By applying a collective electrical field or simultaneously adjusting interdot bias voltages of all double-dot molecule, we get a switchable Ising-like interaction between any two adjacent quantum molecule qubits. The initialization, the single qubit measurement, and the ex…
We propose a scheme to eliminate the effect of non-nearest-neighbor qubits in preparing cluster state with double-dot molecules. As the interaction Hamiltonians between qubits are Ising-model and mutually commute, we can get positive and negative effective interactions between qubits to cancel the effect of non-nearest-neighbor qubits by properly changing the electron charge states of each quantum dot molecule. The total time for the present multi-step cluster state preparation scheme is only doubled for one-dimensional qubit chain and tripled for two-dimensional qubit array comparing with the…
Polyatomic molecular ions contain many desirable attributes of a useful quantum system, including rich internal degrees of freedom and highly controllable coupling to the environment. To date, the vast majority of state-specific experimental work on molecular ions has concentrated on diatomic species. The ability to prepare and readout polyatomic molecules in single quantum states would enable diverse experimental avenues not available with diatomics, including new applications in precision measurement, sensitive chemical and chiral analysis at the single molecule level, and precise studies of…
A single quantum emitter can possess a very strong intrinsic nonlinearity, but its overall promise for nonlinear effects is hampered by the challenge of efficient coupling to incident photons. Common nonlinear optical materials, on the other hand, are easy to couple to but are bulky, imposing a severe limitation on the miniaturization of photonic systems. In this work, we show that a single organic molecule acts as an extremely efficient nonlinear optical element in the strong coupling regime of cavity quantum electrodynamics. We report on single-photon sensitivity in nonlinear signal generati…
We report on a novel experiment to generate non-classical atomic states via quantum non-demolition (QND) measurements on cold atomic samples prepared in a high finesse ring cavity. The heterodyne technique developed for the QND detection exhibits an optical shot-noise limited behavior for local oscillator optical power of a few hundred \muW, and a detection bandwidth of several GHz. This detection tool is used in single pass to follow non destructively the internal state evolution of an atomic sample when subjected to Rabi oscillations or a spin-echo interferometric sequence.
We demonstrate quantum bath engineering for preparation of any orbital state with controllable phase factor of a superconducting flux qubit assisted by a microwave coplanar waveguide resonator. We investigate the polarization efficiency of the arbitrary direction rotating on the Bloch sphere, and obtain an effective Rabi frequency by using the convergence condition of Markovian master equation. The processes of polarization can be implemented effectively in a dissipative environment created by resonator photon loss when the spectrum of the microwave resonator matches with the specially tailore…
State selective preparation and manipulation of discrete-level quantum systems such as atoms, molecules or quantum dots is a the ultimate tool for many diverse fields such as laser control of chemical reactions, atom optics, high-precision metrology and quantum computing. Rabi oscillations are one of the simplest, yet potentially quite useful mechanisms for achieving such manipulation. Rabi theory establishes that in the two-level systems resonant drive leads to the periodic and complete population oscillations between the two system levels. In this paper an analytic optimization algorithm for…
The preparation of a quantum degenerate gas of heteronuclear molecules has been an outstanding challenge. We use path integral Quantum Monte Carlo simulations to understand the role of interactions and finite temperature effects in the protocol currently employed to adiabatically prepare a low-entropy gas of polar molecules in a lattice starting from an ultracold Bose-Fermi mixture. We find that interspecies interactions affect the final temperature of the mixture after the adiabatic loading procedure and detrimentally limit the molecular peak filling. Our conclusions are in agreement with rec…
Mach-Zehnder atom interferometry requires hold-time phase-squeezing to attain readout accuracy below the standard quantum limit. This increases its sensitivity to phase-diffusion, restoring shot-noise scaling of the optimal signal-to-noise ratio, $s_o$, in the presence of interactions. The contradiction between the preparations required for readout accuracy and robustness to interactions, is removed by monitoring Rabi-Josephson oscillations instead of relative-phase oscillations during signal acquisition. Optimizing $s_o$ with a Gaussian squeezed input, we find that hold-time number squeezing …
Rabi frequencies for multiphoton absorption by atoms or molecules that can be characterized as two- or three-level systems are obtained in the cases of single and double laser perturbations. If the ambiguity in the origin of absolute energy is conveniently gauged off in the three-level model, there appears an additional non linear frequency which is originated from the separate evolution of a relative-frequency component induced in the whole system by the simultaneous action of the two perturbations.
We study the growth dynamics of ordered structures of strongly interacting polar molecules in optical lattices. Using dipole blockade of microwave excitations, we map the system onto an interacting spin-1/2 model possessing ground states with crystalline order, and describe a way to prepare these states by non-adiabatically driving the transitions between molecular rotational levels. The proposed technique bypasses the need to cross a phase transition and allows for the creation of ordered domains of considerably larger size compared to approaches relying on adiabatic preparation.
Quantum state preparation plays an equally important role with quantum operations and measurements in quantum information processing. The previous methods of preparing initial state for bulk quantum computation all have inevitable disadvantages, such as, requiring multiple experiments, causing loss of signals, or requiring molecules with restrictive structure. In this work, three kinds of quantum circuits are introduced to prepare the pseudo-pure states of ($n-1$) qubits in the Hilbert space of $n$ coupled spins which merely need the assist of one ancilla spin and two experiments independent o…
Vibronic coupling effects usually manifest themselves in molecules and crystals rather than in an unbound atoms. We theoretically demonstrate the existence of vibronic states in a moving two-level atom exposed to a strong electromagnetic wave. In this case, the Rabi oscillations of the electron density give rise to periodic displacements of the atom center of mass with the Rabi frequency. The periodic displacements mix the Stark split electron levels and lead to the establishment of a channel for energy transfer in the photon-electron-center-of-mass system. Such a channel paves the way for fas…
Coherent population trapping is a well-known quantum phenomenon in a driven $Λ$ system, with many applications across quantum optics. However, when a stochastic bath is present in addition to vacuum noise, the observed trapping is no longer perfect. Here we derive a time-convolutionless master equation describing the equilibration of the $Λ$ system in the presence of additional temporally correlated classical noise, with an unknown decay parameter. Our simulations show a one-to-one correspondence between the decay parameter and the depth of the characteristic dip in the photoluminescence spect…
We investigate both experimentally and theoretically a simple yet more robust and flexible alternative to Rabi oscillation-type biexciton preparation protocols traditionally used for semiconductor quantum dots. The quantum dot is excited by a strong laser pulse positively detuned from the two-photon resonance yielding an on demand initialization of the biexciton state by making use of the phonon-induced thermalization of the photon dressed states. It is shown that for excitation pulses in the picosecond range, a stable and high fidelity of up to $f_{XX}=0.98\pm 0.01$ is reached. Notably, the g…
Preparing molecules at rest and in a highly pure quantum state is a long standing dream in chemistry and physics, so far achieved only for a select set of molecules in dedicated experimental setups. Here, a quantum-limited combination of mass spectrometry and Raman spectroscopy is proposed that should be applicable to a wide range of molecular ions. Excitation of electrons in the molecule followed by uncontrolled decay and branching into several lower energy states is avoided. Instead, the molecule is always connected to rotational states within the electronic and vibrational ground-state mani…
Strong molecule-light interaction enables the control of molecular structures and dynamical processes. A model with strong laser drive is proposed to greatly enhance the intermolecular distance of resonant energy transfer, where the molecules are strongly driven by an optical cavity. The optimal Rabi frequency and quantum yield of energy transfer are observed, resulting from the trade off between dipole-dipole interaction and molecule-cavity coupling. When the strong drive at certain Rabi frequency is applied, a larger spatial range of effective energy transfer and a slower decay rate with the…
The energy states in semiconductor quantum dots are discrete as in atoms, and quantum states can be coherently controlled with resonant laser pulses. Long coherence times allow the observation of Rabi-flopping of a single dipole transition in a solid state device, for which occupancy of the upper state depends sensitively on the dipole moment and the excitation laser power. We report on the robust preparation of a quantum state using an optical technique that exploits rapid adiabatic passage from the ground to an excited state through excitation with laser pulses whose frequency is swept throu…
We propose two schemes for generating the Knill-Lafamme-Milburn (KLM) states of two distant polar molecules (PMs) ensembles respectively in two transmission-line resonators (TLRs) connected by a superconducting charge qutrit (SCQ), and of two SCQs in a TLR, respectively. Both of the schemes are robust against photon decay due to the virtual excitations of the microwave photons of the TLRs, and the spontaneous emission can be suppressed owing to the virtual transitions of the SCQs in the second scheme. In addition, the schemes have high controllability and feasibility under the current availabl…
When an atom strongly couples to a cavity, it can undergo coherent vacuum Rabi oscillations. Controlling these oscillatory dynamics quickly relative to the vacuum Rabi frequency enables remarkable capabilities such as Fock state generation and deterministic synthesis of quantum states of light, as demonstrated using microwave frequency devices. At optical frequencies, however, dynamical control of single-atom vacuum Rabi oscillations remains challenging. Here, we demonstrate coherent transfer of optical frequency excitation between a single quantum dot and a cavity by controlling vacuum Rabi o…
Two coupled-cavity systems, or "photonic dimers", are efficient test-beds for both fundamental optics -the realization of quantum correlated states, Josephson physics, and so forth-, and applications such as optical flip-flop memories. In this work we report on the first observation of nonlinear mode interaction in a photonic dimer formed by two semiconductor photonic crystal coupled nanolasers. For this, we investigate energy transfer between hybrid modes, which manifests as a switching from the blue-detuned (bonding) to the red-detuned (anti-bonding) modes. An mean-field model allows us to e…
Regularized Counterdiabatic Driving for the Quantum Rabi Model
TECNALIA, Basque Research and Technology Alliance (BRTA)（特克拉利亚，巴斯克研究与技术联盟）；University of the Basque Country UPV/EHU（巴斯克大学）；Forschungszentrum Jülich（于利希研究中心）；CSIC（西班牙国家研究委员会）；Instituto de Ciencia de Materiales de Madrid (ICMM), CSIC（马德里材料科学研究所）
We propose a set of subradiant states which can be prepared and detected in a one-dimensional optical lattice. We find that the decay rates are highly dependent on the spatial phases imprinted on the atomic chain, which gives systematic investigations of the subradiance in the fluorescence experiments. The time evolution of these states can have long decay time where up to hundred milliseconds of lifetime is predicted for one hundred atoms. They can also show decayed Rabi-like oscillations with a beating frequency determined by the difference of cooperative Lamb shift in the subspace. Experime…
We study experimentally various physical limitations and technical imperfections that lead to damping and finite contrast of optically-driven Rabi oscillations between ground and Rydberg states of a single atom. Finite contrast is due to preparation and detection errors and we show how to model and measure them accurately. Part of these errors originates from the finite lifetime of Rydberg states and we observe its $n^3$-scaling with the principal quantum number $n$. To explain the damping of Rabi oscillations, we use simple numerical models, taking into account independently measured experime…
Laser cooling and trapping of atoms and atomic ions has led to numerous advances including the observation of exotic phases of matter, development of exquisite sensors and state-of-the-art atomic clocks. The same level of control in molecules could also lead to profound developments such as controlled chemical reactions and sensitive probes of fundamental theories, but the vibrational and rotational degrees of freedom in molecules pose a formidable challenge for controlling their quantum mechanical states. Here, we use quantum-logic spectroscopy (QLS) for preparation and nondestructive detecti…
The strong interaction of individual quantum emitters with resonant cavities is of fundamental interest for understanding light matter interactions. Plasmonic cavities hold the promise of attaining the strong coupling regime even under ambient conditions and within subdiffraction volumes. Recent experiments revealed strong coupling between individual plasmonic structures and multiple organic molecules, but so far strong coupling at the limit of a single quantum emitter has not been reported. Here we demonstrate vacuum Rabi splitting, a manifestation of strong coupling, using silver bowtie plas…
Sub-MHz SWAP spectroscopy of two-level systems in superconducting qubits
Amazon Center for Quantum Computing（亚马逊量子计算中心）；Institute for Quantum Information and Matter, California Institute of Technology（加州理工学院量子信息与物质研究所）；Thomas J. Watson, Sr., Laboratory of Applied Physics, California Institute of Technology（加州理工学院托马斯·J·沃森Sr.应用物理实验室）
We introduce a broadly applicable technique to create nuclear spin singlet states in organic molecules and other many-atom systems. We employ a novel pulse sequence to produce a spin-lock induced crossing (SLIC) of the spin singlet and triplet energy levels, which enables triplet/singlet polarization transfer and singlet state preparation. We demonstrate the utility of the SLIC method by producing a long-lived nuclear spin singlet state on two strongly-coupled proton pairs in the tripeptide molecule phenylalanine-glycine-glycine dissolved in D2O, and by using SLIC to measure the J-couplings, c…
We investigate a nonlinear localization microscopy method based on Rabi oscillations of single emitters. We demonstrate the fundamental working principle of this new technique using a cryogenic far-field experiment in which subwavelength features smaller than $λ$/10 are obtained. Using Monte Carlo simulations, we show the superior localization accuracy of this method under realistic conditions and a potential for higher acquisition speed or a lower number of required photons as compared to conventional linear schemes. The method can be adapted to other emitters than molecules and allows for th…
Organic molecules have recently gained attention as novel sources of single photons. We present a joint experiment--theory analysis of the temperature-dependent emission spectra, zero-phonon linewidth, and second-order correlation function of light emitted from a single molecule. We observe spectra with a zero-phonon-line together with several additional sharp peaks, broad phonon sidebands, and a strongly temperature dependent homogeneous broadening. Our model includes both localised vibrational modes of the molecule and a thermal phonon bath, which we include non-perturbatively, and is able c…
Quantum mechanical phenomena, such as electronic coherence and entanglement, play a key role in achieving the unrivalled efficiencies of light-energy conversion in natural photosynthetic light-harvesting complexes, and triggered the growing interest in the possibility of organic quantum computing. Since biological systems are intrinsically heterogeneous, clear relations between structural and quantum-mechanical properties can only be obtained by investigating individual assemblies. However, single-molecule techniques to access ultrafast coherences at physiological conditions were not available…
The variational quantum eigensolver (VQE) is currently the flagship algorithm for solving electronic structure problems on near-term quantum computers. This hybrid quantum/classical algorithm involves implementing a sequence of parameterized gates on quantum hardware to generate a target quantum state, and then measuring the expectation value of the molecular Hamiltonian. Due to finite coherence times and frequent gate errors, the number of gates that can be implemented remains limited on current quantum devices, preventing accurate applications to systems with significant entanglement, such a…
We investigate the distribution of the number of photons emitted by a single molecule undergoing a spectral diffusion process and interacting with a continuous wave laser field. The spectral diffusion is modeled based on a stochastic approach, in the spirit of the Anderson-Kubo line shape theory. Using a generating function formalism we solve the generalized optical Bloch equations, and obtain an exact analytical formula for the line shape and Mandel's Q parameter. The line shape exhibits well known behaviors, including motional narrowing when the stochastic modulation is fast, and power broad…
Rotational excitation of polar molecules trapped in an optical lattice gives rise to rotational excitons. Here we show that non-linear interactions of such excitons can be controlled by an electric field. The exciton--exciton interactions can be tuned to induce exciton pairing, leading to the formation of biexcitons. Tunable non-linear interactions between excitons can be used for many applications ranging from the controlled preparation of entangled quasiparticles to the study of polaron interactions and the effects of non-linear interactions on quantum energy transport in molecular aggregate…
We analyze a method for preparing low-entropy many-body states in isolated quantum optical systems of atoms, ions and molecules. Our approach is based upon shifting entropy between different regions of a system by spatially modulating the magnitude of the effective Hamiltonian. We conduct two case studies, on a topological spin chain and the spinful fermionic Hubbard model, focusing on the key question: can a "conformal cooling quench" remove sufficient entropy within experimentally accessible timescales? Finite temperature, time-dependent matrix product state calculations reveal that even mod…
We report the realization of a heteronuclear two-atom of $^{87}$Rb-$^{85}$Rb in the ground state of an optical tweezer (OT). Starting by trapping two different isotopic single atoms, a $^{87}$Rb and a $^{85}$Rb in two strongly focused and linearly polarized OT with 4 $μ$m apart, we perform simultaneously three dimensional Raman sideband cooling for both atoms and the obtained 3D ground state probabilities of $^{87}$Rb and $^{85}$Rb are 0.91(5) and 0.91(10) respectively. There is no obvious crosstalk observed during the cooling process. We then merge them into one tweezer via a species-dependen…
Single molecules in solid-state matrices have been proposed as sources of single-photon Fock states back 20 years ago. Their success in quantum optics and in many other research fields stems from the simple recipes used in the preparation of samples, with hundreds of nominally identical and isolated molecules. Main challenges as of today for their application in photonic quantum technologies are the optimization of light extraction and the on-demand emission of indistinguishable photons. We here present Hong-Ou-Mandel experiments with photons emitted by a single molecule of dibenzoterrylene in…
We study coherent photoassociation, phenomena analogous to coherent optical transients in few-level systems, which may take place in photoassociation of an atomic Bose-Einstein condensate but not in a nondegenerate gas. We develop a second-quantized Hamiltonian to describe photoassociation, and apply the Hamiltonian both in the momentum representation and in the position representation (field theory). Solution of the two-mode problem including only one mode each for the atomic and molecular condensates displays analogs of Rabi oscillations and rapid adiabatic passage. A classical version of th…
Preparation of molecular quantum gas promises novel applications including quantum control of chemical reactions, precision measurements, quantum simulation and quantum information processing. Experimental preparation of colder and denser molecular samples, however, is frequently hindered by fast inelastic collisions that heat and deplete the population. Here we report the formation of two-dimensional Bose-Einstein condensates (BECs) of spinning $g-$wave molecules by inducing pairing interactions in an atomic condensate. The trap geometry and the low temperature of the molecules help reducing …
